Experimental confirmation of a predicted porous hydrogen-bonded organic framework
Experimental confirmation of a predicted porous hydrogen-bonded organic framework
Hydrogen-bonded organic frameworks (HOFs) with low densities and high porosities are rare and challenging to design because most molecules have a strong energetic preference for close packing. Crystal structure prediction (CSP) can rank the crystal packings available to an organic molecule based on their relative lattice energies. This has become a powerful tool for the a priori design of porous molecular crystals. Previously, we combined CSP with structure-property predictions to generate energy–structure–function (ESF) maps for a series of triptycene-based molecules with quinoxaline groups. From these ESF maps, triptycene trisquinoxalinedione (TH5) was predicted to form a previously unknown low-energy HOF (TH5-A) with a remarkably low density of 0.374 g cm-3 and three-dimensional (3-D) pores. Here, we demonstrate the reliability of those ESF maps by discovering this TH5-A polymorph experimentally. This material has a high accessible surface area of 3,284 m2 g-1, as measured by nitrogen adsorption, making it one of the most porous HOFs reported to date.
Shields, Caitlin E.
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Wang, Xue
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Fellowes, Thomas
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Clowes, Rob
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Chen, Linjiang
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Day, Graeme M.
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Slater, Anna G.
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Ward, John W.
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Little, Marc A.
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Cooper, Andrew I.
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6 April 2023
Shields, Caitlin E.
b17c5954-b7a2-42c0-ac1c-74ba4ae6c033
Wang, Xue
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Fellowes, Thomas
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Clowes, Rob
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Chen, Linjiang
043ea9b1-b1e0-4de5-9fd9-c0607346151a
Day, Graeme M.
e3be79ba-ad12-4461-b735-74d5c4355636
Slater, Anna G.
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Ward, John W.
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Little, Marc A.
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Cooper, Andrew I.
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Shields, Caitlin E., Wang, Xue, Fellowes, Thomas, Clowes, Rob, Chen, Linjiang, Day, Graeme M., Slater, Anna G., Ward, John W., Little, Marc A. and Cooper, Andrew I.
(2023)
Experimental confirmation of a predicted porous hydrogen-bonded organic framework.
Angewandte Chemie International Edition, [e2023031].
(doi:10.1002/anie.202303167 SECTIONS).
Abstract
Hydrogen-bonded organic frameworks (HOFs) with low densities and high porosities are rare and challenging to design because most molecules have a strong energetic preference for close packing. Crystal structure prediction (CSP) can rank the crystal packings available to an organic molecule based on their relative lattice energies. This has become a powerful tool for the a priori design of porous molecular crystals. Previously, we combined CSP with structure-property predictions to generate energy–structure–function (ESF) maps for a series of triptycene-based molecules with quinoxaline groups. From these ESF maps, triptycene trisquinoxalinedione (TH5) was predicted to form a previously unknown low-energy HOF (TH5-A) with a remarkably low density of 0.374 g cm-3 and three-dimensional (3-D) pores. Here, we demonstrate the reliability of those ESF maps by discovering this TH5-A polymorph experimentally. This material has a high accessible surface area of 3,284 m2 g-1, as measured by nitrogen adsorption, making it one of the most porous HOFs reported to date.
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Angew Chem Int Ed - Experimental Confirmation of a Predicted Porous Hydrogen‐Bonded Organic Framework
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Accepted/In Press date: 4 April 2023
e-pub ahead of print date: 6 April 2023
Published date: 6 April 2023
Additional Information:
Research Funding:
Engineering and Physical Sciences Research Council. Grant Number: EP/V026887/1
Leverhulme Trust. Grant Number: Leverhulme Research Centre for Functional Materials Design Royal Society. Grant Numbers: 201168, Research Professorship
H2020 European Research Council. Grant Number: 856405.
Identifiers
Local EPrints ID: 477518
URI: http://eprints.soton.ac.uk/id/eprint/477518
ISSN: 1433-7851
PURE UUID: daed95c6-d6d9-4703-9108-4b80a104b103
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Date deposited: 07 Jun 2023 17:08
Last modified: 30 Aug 2024 01:45
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Contributors
Author:
Caitlin E. Shields
Author:
Xue Wang
Author:
Thomas Fellowes
Author:
Rob Clowes
Author:
Linjiang Chen
Author:
Anna G. Slater
Author:
John W. Ward
Author:
Marc A. Little
Author:
Andrew I. Cooper
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